19 May 2021

19 May 2021

Review status: this preprint is currently under review for the journal ACP.

Heterogeneity and Chemical Reactivity of the Remote Troposphere defined by Aircraft Measurements

Hao Guo1, Clare M. Flynn2, Michael J. Prather1, Sarah A. Strode3, Stephen D. Steenrod3, Louisa Emmons4, Forrest Lacey4,5, Jean-Francois Lamarque4, Arlene M. Fiore6, Gus Correa6, Lee T. Murray7, Glenn M. Wolfe3,8, Jason M. St. Clair3,8, Michelle Kim9, John Crounse10, Glenn Diskin10, Joshua DiGangi10, Bruce C. Daube11,12, Roisin Commane11,12, Kathryn McKain13,14, Jeff Peischl14,15, Thomas B. Ryerson13,15, Chelsea Thompson13, Thomas F. Hanisco3, Donald Blake16, Nicola J. Blake16, Eric C. Apel4, Rebecca S. Hornbrook4, James W. Elkins14, Eric J. Hintsa13,14, Fred L. Moore13,14, and Steven Wofsy11 Hao Guo et al.
  • 1Department of Earth System Science, University of California, Irvine, CA 92697
  • 2Department of Meteorology, Stockholm University, Stockholm SE-106 91, Sweden
  • 3Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard Space Flight Center, Greenbelt, MD 20771
  • 4Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO 80301
  • 5Department of Mechanical Engineering, University of Colorado, Boulder, CO 80309
  • 6Department of Earth and Environmental Sciences and Lamont-Doherty Earth Observatory, Columbia University, Palisades, NY 10964
  • 7Department of Earth and Environmental Sciences, University of Rochester, Rochester, NY 14611
  • 8Joint Center for Earth Systems Technology, University of Maryland, Baltimore County, Baltimore, MD 21228
  • 9Department of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125
  • 10Atmospheric Composition, NASA Langley Research Center, Hampton VA 23666
  • 11John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138
  • 12Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA 02138
  • 13Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309
  • 14Global Monitoring Division, Earth System Research Laboratory, NOAA, Boulder, CO 80305
  • 15Chemical Sciences Division, National Oceanic and Atmospheric Administration Earth System Research Laboratory, Boulder, CO 80305
  • 16Department of Chemistry, University of California, Irvine, CA 92697

Abstract. The NASA Atmospheric Tomography (ATom) mission built a photochemical climatology of air parcels based on in situ measurements with the NASA DC-8 aircraft along objectively planned profiling transects through the middle of the Pacific and Atlantic Oceans. ATom measured numerous gases and aerosols, particularly the gaseous species driving the chemical budgets of O3 and CH4: i.e., O3, CH4, CO, C2H6, higher alkanes, alkenes, aromatics, NOx, HNO3, HNO4, peroxyacetylnitrate, other organic nitrates, H2O, HCHO, H2O2, and CH3OOH. From the 10 s (2 km) merged observations, a modeling data stream (MDS) based on observations of the core species, consisting of 146,494 distinct air parcels has been constructed from the 4 ATom deployments, providing a continuous data stream for initializing global chemistry models and calculating the 24-hour chemical tendencies. Tendencies derived from 6 chemistry models using the ATom-1 MDS tend to agree and show a highly heterogeneous troposphere where globally 10% of the parcels control as much as 40% of the budget of O3 and CH4. Surprisingly, modeled probability distributions (100-km cells) match ATom statistics (2 km parcels), indicating that the majority of the observed heterogeneity can be resolved with current global chemistry models. On the other hand, the models' own chemical climatologies underestimate O3 production below 4 km in both Pacific and Atlantic basins because they have lower NOX levels than observed.

Hao Guo et al.

Status: open (until 14 Jul 2021)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-405', Anonymous Referee #1, 17 Jun 2021 reply
  • RC2: 'Comment on acp-2021-405', Anonymous Referee #2, 22 Jun 2021 reply

Hao Guo et al.


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Short summary
The recently completed Atmospheric Tomography (ATom) aircraft mission provides a unique, 2-km scale view of the chemical composition of the troposphere. The simultaneous measurement of the most reactive chemical species allows for a simple calculation of the production and loss of ozone and loss of methane at the finest scales of chemical variability.